Polymorphism in the Ruddlesden-Popper Nickelate LaNiO: Discovery of a Hidden Phase with Distinctive Layer Stacking.

We report the discovery of a novel form of Ruddlesden-Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase LaNiO adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO octahedra alternate in a "1313" sequence. Crystals of this new polymorph are described in space group , although we note evidence for a competing variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at ≈ 134 K. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer LaNiO with as high as 80 K above 14 GPa.